Abstract
Due to their simple structure, i.e., two bond species arranged at random on a regular lattice with highest (cubic) symmetry, III-V and II-VI A1-xBxC zincblende pseudobinary semiconductor alloys (SCA) set a benchmark for studying how the physical properties are impacted by disorder in a context of percolation. Over the past two decades, the international scientific consortium behind the current ViSA-IRP has achieved a unified understanding of the lattice dynamics, covering phonons and phonon-polaritons, of cubic-SCA within an original “percolation” framework, more sophisticated than a simplistic VCA, using inelastic light (Raman) scattering (RS) and inelastic neutron scattering (INS) in combination, with ab initio phonon / Raman calculations in support. Within the ViSa-IRP, our consortium will apply its previous experience, gained in the study of well-matched alloys (WMA) and highly mismatched alloys (HMA) with cubic structure, to tackle Zn1‑xMnx-chalcogen magnetic alloys (MA) with lower (hexagonal) symmetry. This will offer an opportunity to investigate how our “percolation-model machinery” may transfer to low-symmetry crystals and, as an anticipated bonus, to extend the picture by probing collective magnetic excitations (magnons).
Partners
- Institute of Physics at the Nicolaus Copernicus University (Toruń, POLOGNE) – crystal growth: Prof. Strzałkowski (project co-coordinator) & Mrs. Marasek;
- Institute of Physics of the Polish Academy of Sciences (IFPAN, Warsaw, POLOGNE) – X-ray diffraction (Prof. Paszkowicz & Dr. Minikayev);
- Bhabha Atomic Research Centre (BARC; Mumbai, INDE) – inelastic neutron scattering: Dr. Rao;
- Departamento de Fisica, Universidade de Aveiro (Aveiro, PORTUGAL) – ab initio Raman calculations: Prof. Torres;
- IMPMC, Institut de Minéralogie, de Physique des Matériaux et de Cosmochimie, Sorbonne Université (Paris) – high-pressure X-ray diffraction and high-pressure/low-temperature Raman scattering : Dr. Polian;
- CRM2, Lab. Cristallographie, Résonance Magnétique et Modélisations, Université de Lorraine (Nancy) – Solid State Nuclear Magnetic Resonance (Dr. Gardiennet & Dr. Kervern);
- LCP-A2MC, Lab. Laboratoire de Chimie et Physique – Approche Multi-Echelle des Milieux Complexes, Université de Lorraine (Metz) : percolation model (Prof. Pagès – project co-coordinator); high-pressure Raman scattering on phonons and phonon-polaritons (prof. Pagès & M. Franchetti); ab initio phonon calculations (Prof. Postnikov); spectroscopic ellipsometry (Prof. En Naciri & Dr. Broch).
Dates
De 2024 à 2027
Contact
en savoir plus…
IRP «Vibrations of Semiconductor Alloys – International Research Partnership» is a 4-years project of a 4-years (2024 – 2027) “wall-less” associated international laboratory supported by «Lorraine Université d’Excellence» as part of the France 2030 Program – reference ANR-15-IDEX-04-LUE and by the «Excellence Initiative – Research University program at Nicolaus Copernicus University in Toruń».
Figure 1 : Cubic-A1-xBxC 10x10x10 supercell at the A-C bond percolation threshold (x=0.19).
Human-size (~1m3, used for teaching purpose and discussion) 11x11x11 zincblende supercell at x=0.19 oriented perpendicular to the high-density / close-packing (111) planes obtained by random A↔B substitution. The dominant B species along with the invariant C sublattice are omitted for better visualization of the spatial organization of the minor A species. This critical composition (x=0.19) corresponds to the first formation of an infinite, wall-to-wall / bottom-to-top, treelike A-C continuum across the lattice, echoed by a singularity in the composition dependence of the Raman frequency in our percolation model. Remarkably, the as-formed A-C continuum at x=0.19 is a pure fractal in that its density (represented by the ratio between the numbers of occupied and available sites in a given cubic box with length L) decreases as L increases according to a universal scaling law. The strict fractal character is lost as soon as departing from x=0.19, by ascending or descending values – cf. D. Stauffer and A. Aharony, in Introduction to Percolation Theory, Chap. 2 (Taylor and Francis, Bristol, 1994).
Overview of ViSA – IRP Consortium
Figure 2 : Overview of the scientific consortium around the VISA – IRP (coordinating teams in grey).
Framework
The ViSA International Relationship Project – ViSA-IRP (cf. Fig. 2) – is basically concerned with the classification/taxonomy of vibration spectra of semiconductor alloys (SCA). Such systems offer a convenient benchmark to investigate how physical properties in general are impacted by disorder (primarily a chemical / substitutional one, in case of alloys). Our view is that the vibration spectra of SCA can be fruitfully assessed at the mesoscopic scale, e.g., within the percolation approach, and not at the macroscopic or microscopic scales where the historical models operate within an overall framework based on the classical virtual crystal approximation (VCA). Generally, our ambition is to achieve a unified understanding of the vibration spectra of SCA within the shift of paradigm from VCA to percolation model, across crystal structures and across collective dynamic excitations (phonons, phonon-polaritons, magnons). This would be both enlightening on the fundamental side and aesthetically rewarding. The current ViSA-IRP will focus on Zn1‑xMnx-VI magnetic alloys (MA) with hexagonal structure, as the very first test case for extension of our percolation approach beyond now well-studied non-magnetic cubic SCA.
Common PhD works
- Dr. A. Chafi – Lorraine University (Dir. O. Pagès, dec. 2008)
Phonons: a natural mesoscope for studying the alloy disorder - Dr. J. Souhabi – Lorraine University (Dir. O. Pagès, co-Dir : A. Postnikov, nov. 2010)
Re-examination of the phonon mode behaviors of the model Ga(As,P) and SiGe alloys : percolation model and ab initio calculations - Dr. R. Hajj Hussein – Lorraine University (Dir. O. Pagès, co-Dir : A. Postnikov, juil. 2014)
Raman study of the (Ge,Si), (Zn,Be)Se and Zn(Se,S) within the percolation model: clustering vs. anticlustering and phonon-polaritons - Dr. H. Dicko – Lorraine University (Dir. O. Pagès, co-Dir : A. Postnikov, june 2018)
Phonon-polaritons/phonons in ZnSe-based mixed crystals with zincblende and wurtzite structures: forward/backward Raman scattering and percolation scheme - Dr. M.B. Shoker – Lorraine University (Dir. O. Pagès, co-Dir : A. Postnikov, dec. 2020)
Raman study of cubic-CdZnSe within the percolation scheme: phonons, phonon-polaritons and high-pressure - Mrs. D. Singh – Nicolaus Copernicus University in Torun (Dir. K. Strzalkowski – PL, co-Dir. O. Pagès – FR, start in feb. 2022)
Growth and characterization of II-VI crystals based on CdTe for the detection of ionizing radiation
Academia Copernicana Interdisciplinary Doctoral School, Torun (Poland)
International of PhD schools at Nicolaus Copernicus University / Academia Copernicana Programme 2nd Run 2021 / European Funds (Knowledge Education Development) - Mr. T. Halhaddad – Lorraine University (Dir. O. Pagès, co-Dir : A. Postnikov, start in oct. 2021)
High-pressure Raman study of ZnTe-based semiconductor alloys - Mr. A. Elmahjoubi – Lorraine University (Dir. O. Pagès, co-Dir. A. Postnikov, start in oct. 2021)
Lattice dynamics of a (new) mixed semiconductor with extreme contrast in bond physical properties: the case of Cd1-xBex(Se or Te) studied by inelastic light/neutron scattering in combination
PhD-LUE (Lorraine Université d’Excellence) funding targeted on international research partnerships - Mrs. M. Mina – Lorraine University (Dir. O. Pagès, co-Dir. K. Strzalkowski, co-Dir. A. Postnikov, start in oct. 2024)
Lattice dynamics of the high-entropy Zn1-xMnxTe magnetic semiconductor alloy – Inelastic light/neutron scattering
Joint PL-FR PhD-LUE (Lorraine Université d’Excellence) funding awarded within the IRP-ViSA project
Common experiments on national instruments
- 4 – 13 Sept. 2009 : INSTITUT LAUE LANGEVIN (proposers : d’Astutto, Pagès, Postnikov & Rao)
Neutron scattering studies of lattice dynamics in the alloy Zn1-xBexSe (x=0.33)
• IN8 beamline (Resp. A. Ivanov): Inelastic neutron scattering - 2011: SYNCHROTRON SOLEIL / Proposal 20110018 (proposers: Hajj Hussein, Pagès & Polian)
Structural studies of Zn1-xBexTe under high pressure
• CRISTAL beamline (Resp. S. Ravy): X-ray diffraction / 19 – 22 dec.
• ODE beamline (Resp. L. Nataf) : EXAFS / 8 – 14 nov. - 29 sept – 4 Oct. 2017: SYNCHROTRON SOLEIL / Proposal 20170371 (proposers: Dicko, Pagès & Polian)
High pressure x-ray diffraction study of the pressure-induced structural transitions of three Zn1 xCdxSe mixed crystals with zincblende (small x values) or wurtzite (large x values) structure at ambient pressure.
• PSICHE beamline (Resp. J.P. Itié): high-pressure X-ray diffraction - 26 – 27 Jan. 2021: SYNCHROTRON SOLEIL / Free time (Polian)
• PSICHE beamline (Resp. J.P. Itié): high-pressure X-ray diffraction - 17 Nov. 2021: SYNCHROTRON SOLEIL / BAG-2021 coordinated by Le Godec (proposers: Alhaddad, Elmahjoubi, Pagès & Polian)
CdZnTe: HP-XRD
• PSICHE beamline (Resp. J.P. Itié): high-pressure X-ray diffraction - 7 – 8 June 2022: SYNCHROTRON SOLEIL / Proposal 20220432 (proposers: Alhaddad, Elmahjoubi, Pagès & Polian)
High pressure X-ray diffraction study of the prospective Cd1-xBexTe mixed crystals (x~0.1) with unusually large contrast in bond length/stiffness
• PSICHE beamline (Resp. J.P. Itié): high-pressure X-ray diffraction - 12 – 20 Sept. 2023 : INSTITUT LAUE LANGEVIN / Proposal 7-01-598 (proposers : Elmahjoubi, Alhaddad, Pagès, Postnikov, Polian & Rao)
Percolation scenario for hexagonal SCA: a test case by applying Inelastic Neutron Scattering (INS) to wurtzite Zn0.67Mg0.33Se
• IN8 beamline (Resp. A. Ivanov): Inelastic neutron scattering - 1 – 28 Fev. 2024: SYNCHROTRON ESRF / Free Time (proposers: Alhaddad, Mina & Pagès)
High-pressure X-ray diffraction on cubic-Zn1-xMnxSe & cubic-Cd1 xHgxTe
• ID15B beamline (Local contact: S. Gallego-Parra): High-pressure X-ray diffraction on single crystals - 24 – 27 March 2024 : INSTITUT LAUE LANGEVIN / Proposal 7-01-598 Follow-up (proposers : Elmahjoubi, Alhaddad, Pagès, Postnikov, Polian & Rao)
Percolation scenario for hexagonal SCA: a test case by applying Inelastic Neutron Scattering (INS) to wurtzite Zn0.94Mg0.06Se
• IN8 beamline (Resp. A. Ivanov): Inelastic neutron scattering
Common publications
Book chapter
- A. Polian, P. Simon and O. Pagès
Chap. 2 ‘Optical Spectroscopy Methods and high-pressure-high-temperature studies’, 67p.
in Thermodynamic Properties of Solids: Experiment and Modeling, Monograph, 322 p.
edited by S.L. Chaplot, R. Mittal and N. Choudhoury, February 2010
WILEY-VCH Verlag GmbH & Co. KGaA, Berlin; SBN-10:3-527-40812-6; ISBN-13:978-3-527-40812-2
Regular publications
- O. Pagès, M. Ajjoun, D. Bormann, C. Chauvet, E. Tournié and J.P. Faurie, Vibrational evidence for a percolative behavior in ZnBeSe. Physical Review B 65, 035213 (2002).
- O. Pagès, M. Ajjoun, T. Tite, D. Bormann, E. Tournié, K.C. Rustagi. Long wave phonons in ZnSe BeSe mixed crystals : Raman scattering and percolation model. Physical Review B 70, 155319/1-10 (2004)
- A. V. Postnikov, O. Pagès, J. Hugel. Lattice dynamics of mixed semiconductors (Be,Zn)Se from first-principles calculations. Physical Review B 71, 115206/1-10 (2005)
- O. Pagès, A. Chafi, D. Fristot, A.V. Postnikov. (Ga,In)P : A standard alloy in the classification of phonon mode behavior. Physical Review B 73, 165206/1-10 (2006)
- A. Chafi, O. Pagès, A.V. Postnikov, J. Gleize, V. Sallet, E. Rzepka, L.H. Li, B. Jusserand, J.C. Harmand. Combined Raman study of InGaAsN from the N-impurity and InGaAs-matrix sides. Applied Physics Letters 91, 51910 (2007)
- O. Pagès, A.V. Postnikov, M. Kassem, A. Chafi, A. Nassour, S. Lang. Unification of the phonon mode behavior in semiconductor alloys: Theory and ab initio calculations. Physical Review B 77, 125208/1-9 (2008)
- A. Postnikov, O. Pagès, J. Souhabi, A. Nassour and J. Hugel. Impurity vibration modes in II-VI and III-V mixed semiconductors. Physica Status Solidi A 206, 1030 (2009)
- O. Pagès, J. Souhabi, A.V. Postnikov and A. Chafi. Percolation versus Cluster models for multimode vibration spectra of mixed crystals: GaAsP as a case study. Physical Review B 80, 035204/1-12 (2009)
- O. Pagès, A.V. Postnikov, A. Chafi, D. Bormann, P. Simon, F. Glas, F. Firszt, W. Paszkowicz and E. Tournié. Non-random Be-to-Zn substitution in ZnBeSe alloys: Raman scattering and ab initio calculations. European Physical Journal B 73, 461 – 469 (2010)
- G. K. Pradhan, C. Narayana, O. Pagès, A. Breidi, J. Souhabi, A.V. Postnikov, F. El Haj Hassan, S. K. Deb, F. Firszt, W. Paszkowicz and A. Shukla. Pressure-induced phonon freezing in the Zn1-xBexSe alloy: A study via the percolation model. Physical Review B 81, 115207/1-6 (2010)
- F. El Hajj Hassan, A. Postnikov, O. Pagès. Structural, electronic, optic and thermal properties of AlxGa1 xAsySb1-y quaternary alloys: First-principles study. Journal of Alloys & Compounds 504, 559 – 565 (2010)
- G. M. Bhalerao, A. Polian, M. Gauthier, J.-P. Itié, F. Baudelet, T. Ganguli, S.K. Deb, J. Mazher, O. Pagès, F. Firszt and W. Paszkowicz. High Pressure x-ray diffraction and extended x-ray absorption fine structure Studies on Ternary Alloy Zn1-xBexSe. Journal of Applied Physics 108, 083533 (2010)
- T. Ganguli, J. Mazher, A. Polian, S.K. Deb, F. Villain, O. Pagès, W. Paszkowicz and F. Firszt. Lattice relaxation in the highly-contrasted Zn1 xBexSe alloy: an extended x-ray absorption fine structure study. Journal of Applied Physics 108, 083539 (2010)
- G. K. Pradhan, C. Narayana, M. N. Rao, M. d’Astuto, S.L. Chaplot, O. Pagès, A. Breidi, J. Souhabi, A.V. Postnikov, S. K. Deb, T. Ganguli, A. Polian, G. Bhalerao, A. Shukla, F. Firszt and W. Paszkowicz. The Phonon Percolation Scheme for Alloys: Extension to the Whole Lattice Dynamics and Pressure-Dependence. Japanese Journal of Applied Physics 50, 05FE02 (2011)
Regular paper following an Invited talk (O. Pagès) at the 17th Int. Conf. on Ternary and Multinary Compounds – ICTMC 17 (Baku – Azebaïdjan, 26 – 30 sept. 2010). - O. Pagès, J. Souhabi, V. J. B. Torres, A.V. Postnikov and K. C. Rustagi. Re-examination of the SiGe Raman spectra – Percolation / one-dimensional-cluster scheme and ab initio calculations. Physical Review B 86, 045201/1-19 (2012)
- O. Pagès, R. Hajj Hussein, and V.J.B. Torres. GeSi Raman spectra vs. clustering-anticlustering: Percolation scheme and ab initio calculations. Journal of Applied Physics 114, 033513/1-15 (2013)
- R. Hajj Hussein, O. Pagès, F. Firszt, W. Paszkowicz and A. Maillard. Near-forward Raman scattering by bulk and surface phonon-polaritons in the model percolation-type ZnBeSe alloy. Applied Physics Letters 103, 071912/1-5 (2013)
- M. N. Rao, D. Lamago, M. d’Astuto, A. Ivanov, A.V. Postnikov, R. Hajj Hussein, T. Basak, S.L. Chaplot, F. Firszt, W. Paszkowicz, S.K. Deb, and O. Pagès. Lattice dynamics of the model percolation-type (Zn,Be)Se alloy: Inelastic neutron scattering, ab initio study and shell model calculations. Physical Review B 89, 155201/1-13 (2014)
- R. Hajj Hussein, O. Pagès, F. Firszt, A. Marasek, W. Paszkowicz, A. Maillard and L. Broch. Near-forward Raman study of a phonon-polariton reinforcement regime in the Zn(Se,S) alloy. Journal of Applied Physics 116, 083511/1-7 (2014)
- R. Hajj Hussein, O. Pagès, S. Doyen-Schuler, H. Dicko, A.V. Postnikov, F. Firszt, A. Marasek, W. Paszkowicz, A. Maillard, L. Broch and O. Gorochov. Percolation-type multi-phonon pattern of Zn(Se,S): Backward/forward Raman scattering and ab initio calculations. Journal of Alloys & Compounds 644, 704-720 (2015)
- H. Dicko, O. Pagès, R. Hajj Hussein, G. Pradhan, C. Narayana, F. Firszt, A. Marasek, W. Paszkowicz, A. Maillard, C. Jobard, L. Broch and F. El Hajj Hassan. Near-forward/high-pressure-backward Raman study of Zn1 xBexSe (x~0.5) – Evidence for percolation behavior of the long (Zn-Se) bond. Journal of Raman Spectroscopy 47, 357-367 (2016)
- R. Hajj Hussein, O. Pagès, A. Polian, A.V. Postnikov, H. Dicko, F. Firszt, K. Strzalkowski, W. Paszkowicz, L. Broch, S. Ravy and P. Fertey. Pressure-induced phonon freezing in the ZnSeS II-VI mixed crystal: phonon-polaritons and ab initio calculations. Journal of Physics: Condensed Matter 28, 205401/1-13 (2016)
Research highlights / JPCM website 27 avril 2016 - H. Dicko, O. Pagès, F. Firszt, K. Strzalkowski, W. Paszkowicz, A. Maillard, C. Jobard and L. Broch. Near-forward Raman selection rules for the phonon-polariton in (Zn,Be)Se alloys. Journal of Applied Physics 120, 185702/1-8 (2016)
- V.J.B. Torres, R. Hajj Hussein, O. Pagès and M.J. Rayson. Clustering/anticlustering effects on the GeSi Raman spectra at moderate (Ge,Si) contents: Percolation scheme vs. ab initio calculations. Journal of Applied Physics 121, 085704/1-12 (2017)
- H. Dicko, O. Pagès, M. B. Shoker, F. Firszt, K. Strzałkowski, A. Maillard, A. Polian, Y. Battie, L. Broch, A. En Naciri, A.V. Postnikov, W. Paszkowicz and J.-P. Itié. Defect-induced ultimately fast volume phonon-polaritons in the wurtzite Zn0.74Mg0.26Se mixed crystal. Scientific Reports 9, 7817 / 1-8 (2019)
- M. B. Shoker, O. Pagès, H. Dicko, V. J. B. Torres, A.V. Postnikov, A. Polian, F. Firszt, K. Strzałkowski, A. EnNaciri, L. Broch, M. N. Rao, R. Rao, A. Maillard and J.-P. Itié. Multi-phonon (percolation) behavior and local clustering of CdxZn1-xSe-cubic mixed crystals (x≤0.3): a Raman – ab initio study. Journal of Applied Physics 126, 105707/1-16 (2019)
- M. B. Shoker, O. Pagès, V. J. B. Torres, A. Polian, J.-P. Itié, G. K. Pradhan, C. Narayana, M. N. Rao, R. Rao, C. Gardiennet, G. Kervern, K. Strzałkowski, and F. Firszt. Phonon-based partition of (ZnSe-like) semiconductor mixed crystals on approach to their pressure- induced structural transition. Scientific Reports 10, 19803 /1-11 (2020)
- M. B. Shoker, T. Alhaddad, O. Pagès, V. J. B. Torres, A.V. Postnikov, A. Polian, R. Hajj Hussein, G. K. Pradhan, C. Narayana, C. Gardiennet, G. Kervern, L. Nataf, S. Ravy, J.-P. Itié, K. Strzałkowski, A. Marasek and F. Firszt. Exceptional phonon point versus free phonon coupling in Zn1 xBexTe under pressure: an experimental and ab-initio Raman study. Scientific Reports 12, 753/1-10 (2022)
- T. Alhaddad, M. B. Shoker, O. Pagès, A.V. Postnikov, V. J. B. Torres, A. Polian, Y. Le Godec, J. P. Itié, L. Broch, M. B. Bouzourâa, A. En Naciri, S. Diliberto, S. Michel, P. Franchetti, A. Marasek and K. Strzałkowski. Raman study of Cd1 xZnxTe phonons and phonon-polaritons – Experiment and ab initio calculations. Journal of Applied Physics 133, 065701 /1-20 (2023)
- A. Elmahjoubi, M. B. Shoker, O. Pagès, V. J.B. Torres, A. Polian, A.V. Postnikov, C. Bellin, K. Beneut, C. Gardiennet, G. Kervern, A. EnNaciri, L. Broch, R. Hajj Hussein, J.-P. Itié, L. Nataf, S. Ravy, P. Franchetti, S. Diliberto, S. Michel, A. Marasek, and K. Strzałkowski. Vibrational-mechanical properties of the highly-mismatched Cd1-xBexTe semiconductor alloy – Experiment and ab initio calculations. Scientific Reports 13, 14571 (2023).
- T. Alhaddad, M.B. Shoker, O. Pagès, A. Polian, V.J.B. Torres, Y. Le Godec, J.-P. Itié, C. Bellin, L. Béneut, S. Diliberto, S. Michel, A. Marasek, and K. Strzałkowski. Multiscale insight into the Cd1-xZnxTe vibrational-mechanical properties – High-pressure experiments and ab initio calculations.
- A. Elmahjoubi, T. Alhaddad, A.V. Postnikov and O. Pages. Comment on Infrared dielectric function of Ga(As,P) semiconductor alloys near the reststrahlen bands (Applied Physics Letters 123, 172102, 2023)